4,277 research outputs found
The nature of the short wavelength excitations in vitreous silica: X-Rays Brillouin scattering study
The dynamical structure factor (S(Q,E)) of vitreous silica has been measured
by Inelastic X-ray Scattering varying the exchanged wavevector (Q) at fixed
exchanged energy (E) - an experimental procedure that, contrary to the usual
one at constant Q, provides spectra with much better identified inelastic
features. This allows the first direct evidence of Brillouin peaks in the
S(Q,E) of SiO_2 at energies above the Boson Peak (BP) energy, a finding that
excludes the possibility that the BP marks the transition from propagating to
localised dynamics in glasses.Comment: 4 pages, 3 Postscript figures. To appear in Physical Review Letter
Vibrational spectrum of topologically disordered systems
The topological nature of the disorder of glasses and supercooled liquids
strongly affects their high-frequency dynamics. In order to understand its main
features, we analytically studied a simple topologically disordered model,
where the particles oscillate around randomly distributed centers, interacting
through a generic pair potential. We present results of a resummation of the
perturbative expansion in the inverse particle density for the dynamic
structure factor and density of states. This gives accurate results for the
range of densities found in real systems.Comment: Completely rewritten version, accepted in Physical Review Letter
Acoustic Nature of the Boson Peak in Vitreous Silica
New temperature dependent inelastic x-ray (IXS) and Raman (RS) scattering
data are compared to each other and with existing inelastic neutron scattering
data in vitreous silica (v-SiO_2), in the 300 - 1775 K region. The IXS data
show collective propagating excitations up to Q=3.5 nm^-1. The temperature
behaviour of the excitations at Q=1.6 nm^-1 matches that of the boson peak
found in INS and RS. This supports the acoustic origin of the excess of
vibrational states giving rise to the boson peak in this glass.Comment: 10 pages and 4 figure
Combining Raman and infrared spectroscopy as a powerful tool for the structural elucidation of cyclodextrin-based polymeric hydrogels
A detailed experimental and theoretical vibrational analysis of hydrogels of b-cyclodextrin nanosponges
(b-CDNS), obtained by polymerization of b-cyclodextrin (b-CD) with the cross-linking agent ethylenediaminetetraacetic
acid (EDTA), is reported here. Thorough structural characterization is achieved by
exploiting the complementary selection rules of FTIR-ATR and Raman spectroscopies and by supporting
the spectral assignments by DFT calculations of the spectral profiles. The combined analysis of the
FTIR-ATR spectra of the polymers hydrated with H2O and D2O allowed us to isolate the HOH bending
of water molecules not involved in symmetrical, tetrahedral environments. The analysis of the HOH
bending mode was carried out as a function of temperature, showing the existence of a supercooled state
of the water molecules. The highest level of cooperativity of the hydrogen bond scheme was reached at a
value of the b-CD/EDTA molar ratio n = 6. Finally, the connectivity pattern of ââuncoupledââ water molecules
bound to the nanosponge backbone was found to be weakened by increasing T. The temperature
above which the population of non-tetracoordinated water molecules becomes predominant turned out
to be independent of the parameter n
Low-frequency dynamics of disordered XY spin chains and pinned density waves: from localized spin waves to soliton tunneling
A long-standing problem of the low-energy dynamics of a disordered XY spin
chain is re-examined. The case of a rigid chain is studied where the quantum
effects can be treated quasiclassically. It is shown that as the frequency
decreases, the relevant excitations change from localized spin waves to
two-level systems to soliton-antisoliton pairs. The linear-response correlation
functions are calculated. The results apply to other periodic glassy systems
such as pinned density waves, planar vortex lattices, stripes, and disordered
Luttinger liquids.Comment: (v2) Major improvements in presentation style. One figure added (v3)
Another minor chang
The crossover from propagating to strongly scattered acoustic modes of glasses observed in densified silica
Spectroscopic results on low frequency excitations of densified silica are
presented and related to characteristic thermal properties of glasses. The end
of the longitudinal acoustic branch is marked by a rapid increase of the
Brillouin linewidth with the scattering vector. This rapid growth saturates at
a crossover frequency Omega_co which nearly coincides with the center of the
boson peak. The latter is clearly due to additional optic-like excitations
related to nearly rigid SiO_4 librations as indicated by hyper-Raman
scattering. Whether the onset of strong scattering is best described by
hybridization of acoustic modes with these librations, by their elastic
scattering (Rayleigh scattering) on the local excitations, or by soft
potentials remains to be settled.Comment: 14 pages, 6 figures, to be published in a special issue of J. Phys.
Condens. Matte
The Raman coupling function in amorphous silica and the nature of the long wavelength excitations in disordered systems
New Raman and incoherent neutron scattering data at various temperatures and
molecular dynamic simulations in amorphous silica, are compared to obtain the
Raman coupling coefficient and, in particular, its low frequency
limit. This study indicates that in the limit
extrapolates to a non vanishing value, giving important indications on the
characteristics of the vibrational modes in disordered materials; in particular
our results indicate that even in the limit of very long wavelength the local
disorder implies non-regular local atomic displacements.Comment: Revtex, 4 ps figure
The evolution of vibrational excitations in glassy systems
The equations of the mode-coupling theory (MCT) for ideal liquid-glass
transitions are used for a discussion of the evolution of the
density-fluctuation spectra of glass-forming systems for frequencies within the
dynamical window between the band of high-frequency motion and the band of
low-frequency-structural-relaxation processes. It is shown that the strong
interaction between density fluctuations with microscopic wave length and the
arrested glass structure causes an anomalous-oscillation peak, which exhibits
the properties of the so-called boson peak. It produces an elastic modulus
which governs the hybridization of density fluctuations of mesoscopic wave
length with the boson-peak oscillations. This leads to the existence of
high-frequency sound with properties as found by X-ray-scattering spectroscopy
of glasses and glassy liquids. The results of the theory are demonstrated for a
model of the hard-sphere system. It is also derived that certain schematic MCT
models, whose spectra for the stiff-glass states can be expressed by elementary
formulas, provide reasonable approximations for the solutions of the general
MCT equations.Comment: 50 pages, 17 postscript files including 18 figures, to be published
in Phys. Rev.
Elastic constant dishomogeneity and dependence of the broadening of the dynamical structure factor in disordered systems
We propose an explanation for the quadratic dependence on the momentum ,
of the broadening of the acoustic excitation peak recently found in the study
of the dynamic structure factor of many real and simulated glasses. We ascribe
the observed law to the spatial fluctuations of the local wavelength of
the collective vibrational modes, in turn produced by the dishomegeneity of the
inter-particle elastic constants. This explanation is analitically shown to
hold for 1-dimensional disordered chains and satisfatorily numerically tested
in both 1 and 3 dimensions.Comment: 4 pages, RevTeX, 5 postscript figure
Inelastic light, neutron, and X-ray scatterings related to the heterogeneous elasticity of glasses
The effects of plasticization of poly(methyl methacrylate) glass on the boson
peaks observed by Raman and neutron scattering are compared. In plasticized
glass the cohesion heterogeneities are responsible for the neutron boson peak
and partially for the Raman one, which is enhanced by the composition
heterogeneities. Because the composition heterogeneities have a size similar to
that of the cohesion ones and form quasiperiodic clusters, as observed by small
angle X-ray scattering, it is inferred that the cohesion heterogeneities in a
normal glass form nearly periodic arrangements too. Such structure at the
nanometric scale explains the linear dispersion of the vibrational frequency
versus the transfer momentum observed by inelastic X-ray scattering.Comment: 9 pages, 2 figures, to be published in J. Non-Cryst. Solids
(Proceedings of the 4th IDMRCS
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